A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li-S Batteries

Kaiqiang Qin; Shi Li; Dean Yen; Weiran Zhang; Zhenzhen Yang; Ethan Phillip Kamphaus; Eric Youngsam Kim; Jinghao Huang; John J. Shea; Enyuan Hu; Lei Cheng; Chunsheng Wang; Chao Luo

doi:10.1021/acsenergylett.4c00859

A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li-S Batteries

Kaiqiang Qin, Shi Li, Dean Yen, Weiran Zhang, Zhenzhen Yang, Ethan Phillip Kamphaus, Eric Youngsam Kim, Jinghao Huang, John J. Shea, Enyuan Hu, Lei Cheng, Chunsheng Wang, Chao Luo

Energy Storage & Conversion

Research output: Contribution to journal › Article › peer-review

Abstract

The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte conditions. Herein, a LiF-rich SEI and a LiF-Li_xN_yO_z coenriched CEI are simultaneously formed by adding ionic liquid (Py₁₃TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. The LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN, therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm^-2) pouch cells under the lean electrolyte conditions (E/S ratio of 5 mL g_SPAN^-1) deliver a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium-sulfur batteries.

Original language	English
Pages (from-to)	3869-3876
Number of pages	8
Journal	ACS Energy Letters
Volume	9
Issue number	8
DOIs	https://doi.org/10.1021/acsenergylett.4c00859
State	Published - Aug 9 2024

Funding

This work was supported by the George Mason University, College of Science Postdoctoral Fellowship and ORIEI Building the Foundation \u2013 Early Stage Seed Funding. The authors also acknowledge the support from the George Mason University Quantum Science & Engineering Center and the startup grant from the University of Miami. We gratefully acknowledge support from the Post Test Facility at Argonne National Laboratory, which is funded by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), under contract DE-AC02-06CH11357. D. Yen and E. Hu are supported by the Assistant Secretary for Energy Efficiency and Renewable Energy (EERE), Vehicle Technology Office (VTO) of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program under contract no. DE-SC0012704. This research used beamline 23-ID-2 (IOS) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. S.L., E.P.K., and L.C. were supported by the Joint Center for Energy Storage Research (JCESR), a U.S. Department of Energy, Energy Innovation Hub. We gratefully acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory.

Funders	Funder number
ORIEI Building the Foundation
George Mason University Quantum Science & Engineering Center
George Mason University
Argonne National Laboratory
Post Test Facility
University of Miami
Joint Center for Energy Storage Research
Office of Science
Brookhaven National Laboratory
Office of Energy Efficiency and Renewable Energy	DE-AC02-06CH11357
U.S. Department of Energy	DE-SC0012704

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10.1021/acsenergylett.4c00859

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title = "A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li-S Batteries",

abstract = "The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte conditions. Herein, a LiF-rich SEI and a LiF-LixNyOz coenriched CEI are simultaneously formed by adding ionic liquid (Py13TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. The LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN, therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm-2) pouch cells under the lean electrolyte conditions (E/S ratio of 5 mL gSPAN-1) deliver a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium-sulfur batteries.",

author = "Kaiqiang Qin and Shi Li and Dean Yen and Weiran Zhang and Zhenzhen Yang and Kamphaus, {Ethan Phillip} and Kim, {Eric Youngsam} and Jinghao Huang and Shea, {John J.} and Enyuan Hu and Lei Cheng and Chunsheng Wang and Chao Luo",

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year = "2024",

month = aug,

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doi = "10.1021/acsenergylett.4c00859",

language = "English",

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T1 - A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li-S Batteries

AU - Qin, Kaiqiang

AU - Li, Shi

AU - Yen, Dean

AU - Zhang, Weiran

AU - Yang, Zhenzhen

AU - Kamphaus, Ethan Phillip

AU - Kim, Eric Youngsam

AU - Huang, Jinghao

AU - Shea, John J.

AU - Hu, Enyuan

AU - Cheng, Lei

AU - Wang, Chunsheng

AU - Luo, Chao

PY - 2024/8/9

Y1 - 2024/8/9

N2 - The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte conditions. Herein, a LiF-rich SEI and a LiF-LixNyOz coenriched CEI are simultaneously formed by adding ionic liquid (Py13TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. The LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN, therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm-2) pouch cells under the lean electrolyte conditions (E/S ratio of 5 mL gSPAN-1) deliver a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium-sulfur batteries.

AB - The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte conditions. Herein, a LiF-rich SEI and a LiF-LixNyOz coenriched CEI are simultaneously formed by adding ionic liquid (Py13TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. The LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN, therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm-2) pouch cells under the lean electrolyte conditions (E/S ratio of 5 mL gSPAN-1) deliver a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium-sulfur batteries.

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A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li-S Batteries

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